Expanding the “Terpenome”: Diterpene Synthases Accept GGPP-Ether Substrates

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-04-11 DOI:10.1021/acscatal.5c0027210.1021/acscatal.5c00272

Viktoria Ravkina, Gerald Dräger, Jörn Droste, Svenja Schwörer, Ahmed Hassanin, Mehdi D. Davari* and Andreas Kirschning*,

引用次数: 0

Abstract

Three geranylgeranyl pyrophosphate derivatives carrying an ether group at different positions within geranylgeranyl pyrophosphate were employed in biotransformations with five diterpene synthases (CotB2, PvHVS, PaFS, Bnd4 and TXS) derived from plants, bacteria and fungi. A total of six new oxygen-containing diterpenoids were isolated and characterized, deepening our knowledge on the substrate promiscuity of diterpene synthases. In addition, the diterpene synthase PvHVS also accepts an ether derivative of farnesyl pyrophosphate and converts it to the same tetrahydrofuran core as found for the analogous extended GGPP substrate. This result further demonstrates that diterpene synthases also exhibit promiscuity toward truncated unnatural substrates.

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扩大“萜烯”：二萜合成酶接受GGPP-Ether底物

利用三种香叶香叶基焦磷酸衍生物，在香叶香叶基焦磷酸的不同位置携带醚基，与来自植物、细菌和真菌的五种二萜合成酶（CotB2、PvHVS、PaFS、Bnd4和TXS）进行生物转化。共分离并鉴定了6个新的含氧二萜，加深了我们对二萜合酶底物混杂性的认识。此外，二萜合成酶PvHVS也接受法尼基焦磷酸的醚衍生物，并将其转化为与类似的扩展GGPP底物相同的四氢呋喃核心。这一结果进一步表明，二萜合成酶对截断的非天然底物也表现出混杂性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.